[1] Absorption by light-absorbing carbon (LAC) particles increases when the carbon is mixed with other material, and this change affects climate forcing. We investigate this increase theoretically over a realistic range of particle sizes. Perfect mixing at the molecular level often overestimates absorption. Assuming that LAC is coated by a concentric shell of weakly absorbing material, we calculate absorption by a range of realistic particle sizes and identify regimes in which absorption behaves similarly. We provide fits to amplification in five regions: (1) small cores and (2) Amplification in region 1 is highest but is physically implausible. Amplification in region 5 is constant at about 1.9 and represents an asymptote for particles with broad size distributions. Because absorption by aggregates is amplified by about 1.3 above spherical particles, and that factor is lost when particles are coated, we suggest that absorption by aged aerosol is about 1.5 times greater than that of fresh aerosol. The rate at which particles acquire sufficient coating to increase their original diameter by 60% is important in determining total absorption during their atmospheric lifetimes. Fitted amplification factors are not very sensitive to assumed refractive index of LAC and can be used even in simple models.

High concentrations of pollution particles, including "soot" or black carbon, exist over the Indian Ocean, but their sources and geographical origins are not well understood. We measured emissions from the combustion of biofuels, used widely in south Asia for cooking, and found that large amounts of carbonaceous aerosols are emitted per kilogram of fuel burnt. We calculate that biofuel combustion is the largest source of black carbon emissions in India, and we suggest that its control is central to climate change mitigation in the south Asian region.

[1] Climatological mean estimates of forest burning and crop waste burning based on broad assumptions of the amounts burned have so far been used for India in global inventories.Here we estimate open biomass burning representative of 1995-2000 from forests using burned area and biomass density specific for Indian ecosystems and crop waste burning as a balance between generation and known uses as fuel and fodder. High-resolution satellite data of active fires and land cover classification from MODIS, both on a scale of 1 km  1 km, were used to capture the seasonal variability of forest and crop waste burning and in conjunction with field reporting. Correspondence in satellite-detected fire cycles with harvest season was used to identify types crop waste burned in different regions. The fire season in forest areas was from February to May, and that in croplands varied with geographical location, with peaks in April and October, corresponding to the two major harvest seasons. Spatial variability in amount of forest biomass burned differed from corresponding forest fire counts with biomass burned being largest in central India but fire frequency being highest in the east-northeast. Unutilized crop waste and MODIS cropland fires were predominant in the western IndoGangetic plain. However, the amounts of unutilized crop waste in the four regions were not strictly proportional to the fire counts. Fraction crop waste burned in fields ranged from 18 to 30% on an all-India basis and had a strong regional variation. Open burning contributes importantly (about 25%) to black carbon, organic matter, and carbon monoxide emissions, a smaller amount (9-13%) to PM 2.5 (particulate mass in particles smaller than 2.5 micron diameter) and CO 2 emissions, and negligibly to SO 2 emissions (1%). However, it cannot explain a large ''missing source'' of BC or CO from India.

Abstract. Delhi, India, routinely experiences some of the world's highest urban particulate matter concentrations. We established the Delhi Aerosol Supersite study to provide long-term characterization of the ambient submicron aerosol composition in Delhi. Here we report on 1.25 years of highly time-resolved speciated submicron particulate matter (PM1) data, including black carbon (BC) and nonrefractory PM1 (NR-PM1), which we combine to develop a composition-based estimate of PM1 (“C-PM1” = BC + NR-PM1) concentrations. We observed marked seasonal and diurnal variability in the concentration and composition of PM1 owing to the interactions of sources and atmospheric processes. Winter was the most polluted period of the year, with average C-PM1 mass concentrations of ∼210 µg m−3. The monsoon was hot and rainy, consequently making it the least polluted (C-PM1 ∼50 µg m−3) period. Organics constituted more than half of the C-PM1 for all seasons and times of day. While ammonium, chloride, and nitrate each were ∼10 % of the C-PM1 for the cooler months, BC and sulfate contributed ∼5 % each. For the warmer periods, the fractional contribution of BC and sulfate to C-PM1 increased, and the chloride contribution decreased to less than 2 %. The seasonal and diurnal variation in absolute mass loadings were generally consistent with changes in ventilation coefficients, with higher concentrations for periods with unfavorable meteorology – low planetary boundary layer height and low wind speeds. However, the variation in C-PM1 composition was influenced by temporally varying sources, photochemistry, and gas–particle partitioning. During cool periods when wind was from the northwest, episodic hourly averaged chloride concentrations reached 50–100 µg m−3, ranking among the highest chloride concentrations reported anywhere in the world. We estimated the contribution of primary emissions and secondary processes to Delhi's submicron aerosol. Secondary species contributed almost 50 %–70 % of Delhi's C-PM1 mass for the winter and spring months and up to 60 %–80 % for the warmer summer and monsoon months. For the cooler months that had the highest C-PM1 concentrations, the nighttime sources were skewed towards primary sources, while the daytime C-PM1 was dominated by secondary species. Overall, these findings point to the important effects of both primary emissions and more regional atmospheric chemistry on influencing the extreme particle concentrations that impact the Delhi megacity region. Future air quality strategies considering Delhi's situation in both a regional and local context will be more effective than policies targeting only local, primary air pollutants.

No abstract

[1] This study focuses on improving source apportionment of carbonaceous aerosol in South Asia and consists of three parts: (1) development of novel molecular marker-based profiles for real-world biofuel combustion, (2) application of these profiles to a year-long data set, and (3) evaluation of profiles by an in-depth sensitivity analysis. Emissions profiles for biomass fuels were developed through source testing of a residential stove commonly used in South Asia. Wood fuels were combusted at high and low rates, which corresponded to source profiles high in organic carbon (OC) or high in elemental carbon (EC), respectively. Crop wastes common to the region, including rice straw, mustard stalk, jute stalk, soybean stalk, and animal residue burnings, were also characterized. Biofuel profiles were used in a source apportionment study of OC and EC in Godavari, Nepal. This site is located in the foothills of the Himalayas and was selected for its well-mixed and regionally impacted air masses. At Godavari, daily samples of fine particulate matter (PM 2.5 ) were collected throughout the year of 2006, and the annual trends in particulate mass, OC, and EC followed the occurrence of a regional haze in South Asia. Maximum concentrations occurred during the dry winter season and minimum concentrations occurred during the summer monsoon season. Specific organic compounds unique to aerosol sources, molecular markers, were measured in monthly composite samples. These markers implicated motor vehicles, coal combustion, biomass burning, cow dung burning, vegetative detritus, and secondary organic aerosol as sources of carbonaceous aerosol. A molecular marker-based chemical mass balance (CMB) model provided a quantitative assessment of primary source contributions to carbonaceous aerosol. The new profiles were compared to widely used biomass burning profiles from the literature in a sensitivity analysis. This analysis indicated a high degree of stability in estimates of source contributions to OC when different biomass profiles were used. The majority of OC was unapportioned to primary sources and was estimated to be of secondary origin, while biomass combustion was the next-largest source of OC. The CMB apportionment of EC to primary sources was unstable due to the diversity of biomass burning conditions in the region. The model results suggested that biomass burning and fossil fuel were important contributors to EC, but could not reconcile their relative contributions.

No abstract

Biomass fuel combustion for residential energy significantly influences both emissions and the atmospheric burden of aerosols in world regions, i.e., east and south Asia. This study reports measurements of climate-relevant properties of particles emitted from biomass fuels widely used for cooking in south Asia, in laboratory experiments simulating actual cooking in the region. Fuel burn rates of 1-2 kg h(-1) for wood species, and 1.5-2 kg h(-1) for crop residues and dried cattle dung, influenced PM2.5 emission factors which were 1.7-2 g kg(-1) at low burn rates but 5-9 gkg(-1) at higher burn rates. Total carbon accounted for 45-55% and ions and trace elements for 2-12% of PM2.5 mass. The elemental carbon (EC) content was variable and highest (22-35%) in particles emitted from low burn rate combustion (wood and jute stalks) but significantly lower (2-4%) from high burn rate combustion (dried cattle dung and rice straw). The mass absorption cross-section (MAC, m2 g(-1)) correlated with EC content for strongly absorbing particles. Weakly absorbing particles, from straw and dung combustion, showed absorption that could not be explained by EC content alone. On average, the MAC of biofuel emission particles was significantly higher than reported measurements from forest fires but somewhat lower than those from diesel engines, indicating potential to significantly influence atmospheric absorption. Both for a given fuel and across different fuels, increased burn rates result in higher emission rates of PM2.5, larger organic carbon (OC) content, larger average particle sizes, and lower MAC. Larger mean particle size (0.42-1.31 microm MMAD) and organic carbon content, than in emissions from combustion sources like diesels, have potential implications for hygroscopic growth and cloud nucleation behavior of these aerosols. These measurements can be used to refine regional emission inventories and derive optical parametrizations, for climate modeling, representative of regions dominated by primary particles from biomass fuel combustion.